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Ultrasensitive Detection and In Situ Imaging of Analytes on Graphene Oxide Analogues Using Enhanced Raman Spectroscopy.

ABSTRACT: We demonstrate how algorithm-improved confocal Raman microscopy (ai-CRM), in combination with chemical enhancement by two-dimensional substrates, can be used as an ultrasensitive detection method for rhodamine (R6G) molecules adsorbed from aqueous solutions. After developing a protocol for laser-induced reduction of graphene oxide, followed by noninvasive Raman imaging, a limit of detection (LOD) of 5 × 10^-10 M R6G was achieved using ai-CRM. An equivalent subnanomolar LOD was also achieved on another graphene oxide analogue -UV/ozone-oxidized graphene. These record-breaking detection capabilities also enabled us to study the adsorption kinetics and image the spatial distribution of the adsorbed R6G. These findings indicate a strong potential for algorithm-improved graphene-enhanced Raman spectroscopy as a facile method for detecting, imaging, and quantifying trace amounts of adsorbing molecules on a variety of 2D substrates.

SUBMITTER: Nair S

PROVIDER: S-EPMC8482369 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Ultrasensitive Detection and In Situ Imaging of Analytes on Graphene Oxide Analogues Using Enhanced Raman Spectroscopy.

Nair Sachin S Gao Jun J Otto Cees C Duits Michael H G MHG Mugele Frieder F

Analytical chemistry 20210914 38

We demonstrate how algorithm-improved confocal Raman microscopy (ai-CRM), in combination with chemical enhancement by two-dimensional substrates, can be used as an ultrasensitive detection method for rhodamine (R6G) molecules adsorbed from aqueous solutions. After developing a protocol for laser-induced reduction of graphene oxide, followed by noninvasive Raman imaging, a limit of detection (LOD) of 5 × 10<sup>-10</sup> M R6G was achieved using ai-CRM. An equivalent subnanomolar LOD was also ach ...[more]

PMID: 34517698

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Project description:In this study, a widely used colloid of Creighton AgNPs (ORI, 1-100 nm, mostly ≤ 40 nm, ∼10 μg mL-1) was rapidly manipulated via tangential flow filtration (TFF) for highly reproducible surface-enhanced (resonance) Raman spectroscopy (SE(R)RS) experiments down to the single-molecule (SM) level. The quasi-spherical AgNPs were size-selected, purified, and concentrated in two TFF fractions of a cutoff diameter of ∼40 nm: AgNP ≤ 40 (∼900 μg mL-1) and AgNP ≥ 40 (∼100 μg mL-1). The SE(R)S-based sensing capabilities of the two TFF fractions were then tested under pre-resonance (632.8 nm) and resonance (532.1 nm) excitation conditions for rhodamine 6G (R6G, 10-6-10-15 M). Both TFF isolates, AgNP ≤ 40 and AgNP ≥ 40, were more effective in adsorbing the R6G analyte (≥91%) than the original colloid (≥78%) at submonolayer coverages. Furthermore, the surface enhancement factors (SEF) of the two TFF fractions were markedly superior to those of ORI under all excitation conditions. SERS at 632.8 nm: only AgNP ≥ 40 enabled the detection of R6G at 10-9 M and produced the largest SEF (2.1 × 106). SE(R)RS and SM-SERRS at 532.1 nm: AgNP ≥ 40 gave rise to the largest SEF values (2.5 × 1010) corresponding to the SM regime down to 10-15 M of R6G. Nevertheless, AgNP ≤ 40 compensated for the size-dependence of the electromagnetic enhancements by an increase in the silver concentration, which led to SEF values comparable to those of AgNP ≥ 40 through additional resonance enhancements. TFF resulted into a ∼100-fold increase (AgNP ≤ 40) in the number of negatively charged AgNPs that were available to electrostatically bridge R6G cations and form SERRS "hot-spots" (AgNP-R6G-AgNP) within the focal volume. Evidently, the interplay between AgNP size, AgNP concentration, and excitation wavelength governs the SE(R)RS enhancements. This study demonstrated that TFF can facilitate the ecofriendly isolation of spherical AgNPs of controlled morphological and plasmonic properties for further enhancing their sensing capabilities as SE(R)RS substrates.

Dataset Information

Ultrasensitive Detection and In Situ Imaging of Analytes on Graphene Oxide Analogues Using Enhanced Raman Spectroscopy.

Publications

Ultrasensitive Detection and In Situ Imaging of Analytes on Graphene Oxide Analogues Using Enhanced Raman Spectroscopy.

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